Organo-lead halide perovskites' attractive optical and electrical properties has given rise to an increased interest in fabricating optoelectronic devices based on organo-lead halide perovskites. For instance, organo-lead halide perovskite polycrystalline thin films have been explored, but the small grain size and presence of grain boundaries has limited the performance and application of organo-lead halide perovskite polycrystalline thin films in optoelectronic devices. While the larger grain sizes and fewer grain boundaries of bulk single crystals sparked interest in perovskite bulk single crystals, the performance of optoelectronic devices based on perovskite bulk single crystals has been inferior to those based on perovskite polycrystalline films due to high surface trap densities and uncontrollable crystal thickness.